Stabilizing the highly active RuO_(2) electrocatalyst for the oxygen evolution reaction(OER)is critical for the application of proton exchange membrane water electrolysis,but this remains challenging due to the inevit...Stabilizing the highly active RuO_(2) electrocatalyst for the oxygen evolution reaction(OER)is critical for the application of proton exchange membrane water electrolysis,but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments.Herein,we describe constructing Ru-O-La asymmetric configurations into RuO_(2) via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers.Specifically,the as-prepared optimal La_(0.1)Ru_(0.9)O_(2) shows a low overpotential of 188 mV at 10 mA cm^(-2),a high mass activity of 251 A gRu^(-1) at 1.6 V vs.reversible hydrogen electrode(RHE),and a long-lasting durability of 63 h,far superior to the 8 h achieved by standard RuO_(2).Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO_(2).More importantly,electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru,thus preventing the over-oxidation of Ru.In addition,electron redistribution tunes the Ru 4d band center’s energy level,which optimizes the adsorption and desorption of oxygen intermediates.This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO_(2)-based acidic OER electrocatalysts.展开更多
There is an urgent need to develop innovative electrochemical energy storage devices that can offer high energy density,long lifespan,excellent rate capability,and improved security.For the electrochemical system,the ...There is an urgent need to develop innovative electrochemical energy storage devices that can offer high energy density,long lifespan,excellent rate capability,and improved security.For the electrochemical system,the electrode interphase,namely the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)play crucial roles in the operating mechanism,kinetics,and overall performance of the battery.However,the in-depth investigation of the unstable and complex electrode interphase is limited by the unavoidable air and moisture contact during the material transfer process and probable high-energy radiation damage in the characterization procedure.Recently,cryogenic techniques and in situ techniques have been developed and applied in the electrode interphase research to settle the radiation damage and air erosion,respectively.However,there has not been a special review that summarizes the relevant methods,so a systematic review is very important to accelerate the development.In this review,we summarize these two state-of-the-art methods,including their working principle,characterization process,advantages,and applications in electrode interphase analysis.And the integrative techniques,which are considered as the future development perspectives,are also discussed.This review can provide important directions for next-generation characterization techniques and strategies to effectively analyze the electrode interphase for advanced batteries.展开更多
Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy.Electrocatalytic reactions occur at the interface of catalysts,where the physicochemical ...Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy.Electrocatalytic reactions occur at the interface of catalysts,where the physicochemical properties of the catalyst surface play a dominant role.In particular,the electron spin behavior on the catalyst surface has a decisive impact on the catalytic reaction process.This review initially introduces the definition of electron spin and methods for spin manipulation.Furthermore,we summarize the advanced characterization methods of electron spin.Then,we review the latest research advancements on the spin effect in the oxygen reduction reaction,oxygen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction.The catalytic mechanisms of spin manipulation in these four reactions are thoroughly discussed.Finally,we propose key directions for the future development of spin effects in the field of electrocatalysis.This review contributes to a deeper understanding of the micromechanisms in electrocatalytic reactions.展开更多
The authors regret an inadvertent error in Fig.3a where a methyl group was drawn as an ethyl group in the trimethyl phosphate(TMP)structure,resulting in ethyl dimethylphosphate.This unintentional oversight occurred du...The authors regret an inadvertent error in Fig.3a where a methyl group was drawn as an ethyl group in the trimethyl phosphate(TMP)structure,resulting in ethyl dimethylphosphate.This unintentional oversight occurred during graphic preparation.A revised structure is provided here.展开更多
With issues of energy security and environmental crisis intensifying,we urgently need to develop energy storage systems with high energy density and high safety.Zinc–air batteries have attracted extensive attention f...With issues of energy security and environmental crisis intensifying,we urgently need to develop energy storage systems with high energy density and high safety.Zinc–air batteries have attracted extensive attention for their energy density,safety,and low cost,but problems with the zinc anode—such as hydrogen evolution,corrosion,passivation,dendrite proliferation,and deformation—have led to zinc–air batteries with low Coulombic efficiency and short cycle life;these remain the key obstacles hindering the batteries’further development.In this review paper,we briefly describe the reaction mechanism of zinc–air batteries,then summarize the strategies for solving the key issues in zinc anodes.These approaches are divided into three aspects:structural designs for the zinc anode;interface engineering;and electrolyte selection and optimization.We finish by offering some suggestions for future research directions to improve the zinc anode in zinc–air batteries.展开更多
Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance.Compared to single-atom catalysts,those incorporating both single atoms and cluster...Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance.Compared to single-atom catalysts,those incorporating both single atoms and clusters exhibit superior catalytic activity.However,the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood.In this study,we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method.Y doping facilitated the formation of Mn clusters and optimized the d-band center of Mn through a unique synergy effect,thereby reducing energy barriers and enhancing the reaction kinetics.Additionally,the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N_(₃)coordination structures,resulting in excellent oxygen reduction reaction(ORR)performance.Consequently,the MnY/NC catalyst demonstrated a half-wave potential(E_(₁/₂))of 0.90 V and maintained stability in 0.1 M KOH,outperforming both Mn/NC and Pt/C.This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems,effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the“remote synergy effect”in heterogeneous catalysis.展开更多
The integration of surface plasmons with catalysis has opened a new frontier in the field of chemical energy conversion,offering unprecedented opportunities for enhancing reaction activity and selectivity.This review ...The integration of surface plasmons with catalysis has opened a new frontier in the field of chemical energy conversion,offering unprecedented opportunities for enhancing reaction activity and selectivity.This review delves into the optical properties of plasmonic materials,the intricate mechanisms of plasmon-assisted chemical reactions(PACRs),and the fabrication of plasmonic catalysts,highlighting the significance of the structure–performance relationship.The mechanisms of PACRs are summarized to understand their synergistic contributions to reactions.The review further examines modern experimental strategies for characterizing surface plasmon resonance properties,including scanning probe microscope,in situ spectroscopy,and ultrafast laser pump-probe techniques,which provide real-time,dynamic insights into molecular interactions and structural changes with high spatial and temporal resolution.We conclude by outlining the challenges and future prospects for PACRs,emphasizing the need for innovative strategies to fully exploit the potential of PACRs for sustainable energy conversion and environmental remediation.展开更多
Bismuth vanadate(BiVO_(4))is a promising photoanode material for photoelectrochemical(PEC)water oxidation.However,its performance is greatly hindered by poor bulk and interfacial charge transfer.Herein,to address this...Bismuth vanadate(BiVO_(4))is a promising photoanode material for photoelectrochemical(PEC)water oxidation.However,its performance is greatly hindered by poor bulk and interfacial charge transfer.Herein,to address this issue,iron doped vanadyl phosphate(Fe:VOPO_(4))was grafted on molybdenum doped BiVO_(4)(Mo:BiVO_(4))for significantly enhancing charge transfer and oxygen evolution kinetics simultaneously.Consequently,the resultant Fe:VOPO_(4)/Mo:BVO_(4) photoanode exhibits a remarkable photocurrent density of 6.59 mA cm^(-2) at 1.23 V versus the reversible hydrogen electrode(VRHE)under AM 1.5G illumination,over approximately 5.5 times as high as that of pristine BiVO_(4).Systematic studies have demonstrated that the hopping activation energy of small polarons is significantly reduced due to the Mo doping,resulting in accelerated bulk charge transfer.More importantly,the deposition of Fe:VOPO_(4) promotes the interfacial charge transfer between Mo:BiVO_(4) and Fe:VOPO_(4) via the construction of V-O-V and P-O bonds,in addition to facilitating water splitting kinetics.This work provides a general strategy for optimizing charge transfer process,especially at the interface between photoanodes and cocatalysts.展开更多
Solid-state lithium battery(SSLB)is considered as one of the promising candidates for next-generation power batteries due to high safety,unprecedented energy density and favorable adaptability to high pression and tem...Solid-state lithium battery(SSLB)is considered as one of the promising candidates for next-generation power batteries due to high safety,unprecedented energy density and favorable adaptability to high pression and temperature.However,the system of solid electrolyte(SE),as one of the most important components in SSLB,is usually plagued by clumsy ionic transport,leading to poor rate performance of the SSLBs.Herein,a unique perspective is proposed to re-examine the ion-transport behavior in lithium conductors by tracing Liþat multiscale,including microscopic,mesoscopic and macroscopic scales.The multi-scale ion-transport mechanisms and corresponding characterization techniques are analyzed in depth.Furthermore,some strategies of structure design to improve ion-transport kinetics at corresponding scales are elaborated systematically,involving the modulation of microscopic homogeneous structure,mesoscopic heterogeneous structure and macroscopic structures,etc.The proposed generalized rules for SEs are expected to construct a close link from mechanism-structure-characterization to high performances for SSLBs.展开更多
Black phosphorus(BP)anode with high capacity(2596 mAh g^(-1))and suitable lithiation potential(0.7 V vs.Li^(+)/Li)is an ideal candidate for high-energy-density and high-safety lithium-ion batteries,however,the practic...Black phosphorus(BP)anode with high capacity(2596 mAh g^(-1))and suitable lithiation potential(0.7 V vs.Li^(+)/Li)is an ideal candidate for high-energy-density and high-safety lithium-ion batteries,however,the practical implementation is greatly limited by its slow reaction kinetics and huge volume expansion.Here,inspired by nature,liquid metal(LM)is explored as a self-heal agent,which can well stabilize the BP anode through buffering the volumetric expansion and re-activating“dead P and Li x P”.Moreover,LM also acts as a good catalyst,which can adjust Li ion concentration and reduce the activation energy of delithiation reaction,thus prolonging the cycling life.Therefore,the LM modified BP/graphite(G)composite delivers an excellent high-rate performance of 1123 mAh g^(-1)at 4 C with 80.0%capacity retention after 200 cycles,a superior wide-temperature performance of 1547.5 mAh g^(-1)and 569.0 mAh g^(-1)at 50℃and-20℃,respectively.展开更多
Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space,which are crucial for the advancement of metaverse applications.However,traditional hardware solutions,reliant on opt...Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space,which are crucial for the advancement of metaverse applications.However,traditional hardware solutions,reliant on optical cameras or inertial sensors,are hampered by privacy concerns,spatial limitations,high costs,and calibration challenges.Here,we propose AI-enabled smart clothing that seamlessly integrates triboelectric strain-sensing fibers(TSSFs)and AI algorithms with commercial fitness suits to achieve precise dynamic 3D reconstruction of body movement.TSSFs enable the dynamic capture of body postures and excel in sensitivity,linearity,and strain range,while maintaining mechanical stability,temperature resilience,and washability.The integrated algorithms accurately decouple posture signals—distinguishing between similar postures with the 1D-CNN algorithm,compensating for body-shape differences via a calibration algorithm,and determining spatial elements for avatar reconstruction using a decision-tree algorithm.Finally,leveraging Unity-3D,we achieve ultra-accurate dynamic 3D avatars with a joint angle error of<3.63°and demonstrate their effectiveness using VR fitness and enter-tainment applications,showing how they can offer users standardized yet engaging experiences.展开更多
The Li-O_(2) battery(LOB)has attracted growing interest,including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity.However,a series of challenge...The Li-O_(2) battery(LOB)has attracted growing interest,including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity.However,a series of challenges have seriously hindered LOB development,such as sluggish kinetics during the oxygen reduction and oxygen evolution reactions(ORR/OER)at the cathode,the formation of lithium dendrites,and undesirable corrosion at the lithium metal anode.Herein,we propose a strategy based on the ultra-low loading of atomic Ni catalysts to simultaneously boost the ORR/OER at the cathode while stabilizing the Li metal anode.The resultant LOB delivers a superior discharge capacity(>16,000 mAh g^(-1)),excellent long-term cycling stability(>200 cycles),and enhanced high rate capability(>300 cycles@500 mA g^(-1)).The working mechanisms of these atomic Ni catalysts are revealed through carefully designed in situ experiments and theoretical calculations.This work provides a novel research paradigm for designing high-performance LOBs that are useable in practical applications.展开更多
Aqueous zinc-ion batteries(ZIBs)represent a promising solution for“beyond-lithium-ion”chemistries,but certain problems hinder their further development,especially when conventional aqueous electrolytes are involved....Aqueous zinc-ion batteries(ZIBs)represent a promising solution for“beyond-lithium-ion”chemistries,but certain problems hinder their further development,especially when conventional aqueous electrolytes are involved.Hydrogel polymer electrolytes(HPEs)offer opportunities to circumvent these issues.This review aims to provide a fundamental understanding of how to design better HPEs for high-performing ZIBs,through critically analyzing the recent literature.Concerns regarding HPEs’mechanical,interfacial,and electrochemical characteristics are addressed,followed by in-depth insights into their underlying mechanisms.Possibilities for practical applications of HPEs are also discussed.展开更多
Wearable tactile sensing systems with bionic designs holds significant promise for environmental interactions and human–machine communication.Triboelectric sensing technology plays a vital role in acquiring and quant...Wearable tactile sensing systems with bionic designs holds significant promise for environmental interactions and human–machine communication.Triboelectric sensing technology plays a vital role in acquiring and quantifying tactile signals.Conventional elastic sensing materials,however,lack damping performance and are easily damaged by vibrations,leading to sensor failure.To address this challenge,our study proposes a highly damping triboelectric gel based on a hydrogen bonding assisted microphase separation strategy.In microphase separation,the soft phase provides the viscoelasticity needed for the gel,while the hard phase dissipates shock energy.This energy dissipation mechanism enables the gel to achieve excellent damping performance(tanδ=0.68 at 1Hz),skin-like softness(Young’s modulus of 130 kPa),and stretchability(>900%).The resulting self-damping tactile patch effectively absorbs and dissipates external vibrations,ensuring a stable and reliable wearable tactile sensing device.This work provides new insights into the application of triboelectric gels in wearable electronics.展开更多
Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era.Different from traditional methods,this work proposes a hyb...Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era.Different from traditional methods,this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning,which is used to rapidly and robustly predict polarization-free incremental capacity analysis(ICA)curves in minutes,and physical modeling,which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves.Only measured charging current and voltage signals are used.Results demonstrates that 11 points collected at any starting state-of-charge(SOC)in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error(RMSE)of 0.2774 Ah/V.Accordingly,battery status can be accurately elevated based on their degradation at both macro and electrode levels.Through transfer learning,such a method can also be adapted to different battery chemistries,indicating the enticing potential for wide applications.展开更多
The development of low-cost and efficient electrocatalysts for oxygen evolution reaction(OER)in acid electro-lytes is critical to the widespread implementation of proton electrolyte membrane water electrolyzers(PEMWE)...The development of low-cost and efficient electrocatalysts for oxygen evolution reaction(OER)in acid electro-lytes is critical to the widespread implementation of proton electrolyte membrane water electrolyzers(PEMWE)towards carbon neutralization.Noble metal Ir-and Ru-based materials are state-of-the-art catalysts but still suffer from prohibitive price and scarcity.In this context,a variety of noble metal-free catalysts have been developed to decrease the cost of PEMWE.In this review,we first summarize the activity expression mechanism and stability issues for non-precious metal catalysts,highlighting the origins of performance degradation and the possible mitigation strategies.Then,we systematically review several recently developed noble metal-free catalysts,focusing on the design rationale and the structure-performance relation.Finally,the development prospects of non-noble metal catalysts are prospected,with the potential challenges for practical applications presented.展开更多
In the development of sustainable lithium-ion batteries,achieving the efficient and cost-effective recycling of all components,particularly spent graphite(SG)anodes,has become a critical requirement.While considerable...In the development of sustainable lithium-ion batteries,achieving the efficient and cost-effective recycling of all components,particularly spent graphite(SG)anodes,has become a critical requirement.While considerable ef-forts have been devoted to recovering and reusing SG materials under conventional conditions,limited attention has been given to recycling under extreme conditions.This review systematically elucidates the main failure mechanisms of graphite anodes,including lithium plating and dendrite formation,solid electrolyte interface film failure,structural degradation,and current collector corrosion,with a particular focus on low-temperature and fast-charging conditions.As a contribution toward optimizing resource utilization,this review comprehensively summarizes the industrial perspective on strategies for recycling SG anodes,which aim to produce high-purity regenerated graphite(RG)powders.We also analyze current methods for modifying RG,such as structural reconstruction and surface reconditioning,to bring added value to modified RG materials.A detailed examination of the technical challenges in SG recycling and RG upgrading is presented,offering guidance for the future development of graphite upcycling technologies.This review also provides valuable insights into achieving high efficiency,intelligence,and sustainability in graphite utilization.展开更多
The invention of aqueous Zn batteries(AZBs)traces back to the eighteenth century.Recently,however,AZBs have been undergoing a renaissance due to the urgent need for renewable energy storage devices that are intrinsica...The invention of aqueous Zn batteries(AZBs)traces back to the eighteenth century.Recently,however,AZBs have been undergoing a renaissance due to the urgent need for renewable energy storage devices that are intrinsically safe,inexpensive,and environmentally benign.The escalating demand for high-energy,fast-charging AZBs,particularly in grid-scale energy storage systems,necessitates a profound exploration of the fundamental aspects of electrode chemistries.In particular,a comprehensive understanding from the viewpoints of thermodynamics and kinetics is crucial,with the aim of advancing the development of next-generation AZBs that have high power and energy densities.However,clarification about the fundamental issues in AZB chemistry has yet to be ach-ieved.This review offers a thorough exploration of the thermodynamics and dynamic mechanisms at the anode and cathode,with the aim of helping researchers achieve high-performance AZBs.The inherent challenges and corresponding strategies related to electrode thermodynamic and dynamic optimization are summarized,fol-lowed by insights into future directions for developing high-energy,fast-charging AZBs.We conclude by considering the future prospects for AZBs and offering recommendations for making further advancements in discovering new redox chemistries,optimizing electrode architectures,and achieving integrated battery designs,all of which are considered essential and time-sensitive for making high-energy,fast-charging,and durable AZBs a reality.展开更多
Hard carbon(HC)anodes in sodium-ion batteries(SIBs)are prized for their high capacity,durability,costefficiency,environmental sustainability,and safety.The metallic ash elements in HCs inevitably affect the overall pe...Hard carbon(HC)anodes in sodium-ion batteries(SIBs)are prized for their high capacity,durability,costefficiency,environmental sustainability,and safety.The metallic ash elements in HCs inevitably affect the overall performance of SIBs,however,the unclear role of metallic ash elements during carbonization and the electrochemical sodium storage process presents challenges for advancing HC design concepts.In this review,the traditional role of metallic ash element realized in the past and the deep understanding by a new sight from the view of intrinsic types in precursor matrix are initially introduced.Subsequently,the effect of catalyzing graphitization degree,constructing pore structure,tuning SEI formation and tailoring defects of the HCs regulated by extrinsic factors introduced through experimental conditions in recent years are comprehensively summarized.Additionally,future development prospects and perspectives on the research about metallic ash element in HC are also briefly outlined.It is believed that this review can deliver noteworthy viewpoints by introducing metallic ash elements,for the continued development of adjusting the microstructure of HCs at the nanoscale to actualize highperformance SIBs.展开更多
Affordable,easily recycled organics with electroactive centers have drawn attention in the pursuit of high-performance aqueous zinc organic batteries(AZOBs).However,intrinsic barriers such as high solubility,unde-sira...Affordable,easily recycled organics with electroactive centers have drawn attention in the pursuit of high-performance aqueous zinc organic batteries(AZOBs).However,intrinsic barriers such as high solubility,unde-sirable potential,and inferior conductivity hinder their further development.To this end,we have designed an advanced cathode material for AZOBs,comprising an n-type polymer with a three-dimensional(3D)building block(HAT-TP)formed by polymerizing 2,3,6,7,10,11-hexacyano-1,4,5,8,9,12-hexazepenanthrene(HAT-CN)and 3D 2,3,6,7,14,15-hexaaminotriptycene(THA-NH 2).The introduction of a 3D architecture not only bolsters the insolubility but also exposes redox-active sites for cation coordination,while the material's extended conjugated system promotes electronic delocalization to increase the redox potential and conductivity.As a result,a HAT-TP battery exhibits a notable initial discharge voltage of 1.32 V at 0.1 A g^(-1),followed by a midpoint voltage of 1.17 V.Remarkably,an ultrastable capacity retention ratio of up to 93.4%is achieved,even after 40,000 cycles at 5 A g^(-1).Theoretical simulations reveal that the elevated discharge potential results from the strong electronic delocalization of HAT-TP,which improves the affinity with cations.Ex situ characterizations and theoretical calculations verify that the reversible Zn^(2+)/H^(+)co-storage mechanism involves only electroactive C=N sites and the best possible coordination paths between them.展开更多
基金support from the National Key Technology R&D Program of China(2022YFB3504302,2022YFC3-901503)Natural Science Foundation and Overseas Talent Projects of Jiangxi Province(20232BAB214025,20232BCJ25044)Self-deployed Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(E355F003).
文摘Stabilizing the highly active RuO_(2) electrocatalyst for the oxygen evolution reaction(OER)is critical for the application of proton exchange membrane water electrolysis,but this remains challenging due to the inevitable over-oxidation of Ru in harsh oxidative environments.Herein,we describe constructing Ru-O-La asymmetric configurations into RuO_(2) via a facile sol-gel method to tailor electron redistribution and thereby eliminate the over-oxidation of Ru centers.Specifically,the as-prepared optimal La_(0.1)Ru_(0.9)O_(2) shows a low overpotential of 188 mV at 10 mA cm^(-2),a high mass activity of 251 A gRu^(-1) at 1.6 V vs.reversible hydrogen electrode(RHE),and a long-lasting durability of 63 h,far superior to the 8 h achieved by standard RuO_(2).Experiments and density functional theory calculations jointly reveal that the Ru-O-La asymmetric configuration could trigger electron redistribution in RuO_(2).More importantly,electron transfer from La to Ru via the Ru-O-La configuration could lead to increased electron density around Ru,thus preventing the over-oxidation of Ru.In addition,electron redistribution tunes the Ru 4d band center’s energy level,which optimizes the adsorption and desorption of oxygen intermediates.This work offers an effective strategy for regulating electronic structure to synergistically boost the activity and stability of RuO_(2)-based acidic OER electrocatalysts.
基金supported by the National Nature Science Foundation of China(No.22272205,No.22279164)Hunan Provincial Nature Science Foundation of China(No.2022JJ30685)+4 种基金Hunan Provincial Science and Technology Plan Project of China(No.2017TP1001)the Science and Technology Innovation Program of Hunan Province(2023RC3058)the Scientific and Technological Research Program of Chongqing Municipal Education Commission(No.KJZD-M202101401)Aid Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Provincesupport from Science and Technology Innovation Team for Photovoltaic Power and Energy Storage Battery Key Technologies at General University in Hunan Province.D.S.acknowledges support from Young Elite Scientists Sponsorship Program by CAST(No.YESS20220432).
文摘There is an urgent need to develop innovative electrochemical energy storage devices that can offer high energy density,long lifespan,excellent rate capability,and improved security.For the electrochemical system,the electrode interphase,namely the cathode electrolyte interphase(CEI)and solid electrolyte interphase(SEI)play crucial roles in the operating mechanism,kinetics,and overall performance of the battery.However,the in-depth investigation of the unstable and complex electrode interphase is limited by the unavoidable air and moisture contact during the material transfer process and probable high-energy radiation damage in the characterization procedure.Recently,cryogenic techniques and in situ techniques have been developed and applied in the electrode interphase research to settle the radiation damage and air erosion,respectively.However,there has not been a special review that summarizes the relevant methods,so a systematic review is very important to accelerate the development.In this review,we summarize these two state-of-the-art methods,including their working principle,characterization process,advantages,and applications in electrode interphase analysis.And the integrative techniques,which are considered as the future development perspectives,are also discussed.This review can provide important directions for next-generation characterization techniques and strategies to effectively analyze the electrode interphase for advanced batteries.
基金supported by the National Natural Science Foundation of China(Nos:22271018,22309012,and 22302013)the NSF of Guangdong Province(2023A1515010554).
文摘Building highly reactive electrocatalysts is of great significance for addressing the energy crisis and developing green energy.Electrocatalytic reactions occur at the interface of catalysts,where the physicochemical properties of the catalyst surface play a dominant role.In particular,the electron spin behavior on the catalyst surface has a decisive impact on the catalytic reaction process.This review initially introduces the definition of electron spin and methods for spin manipulation.Furthermore,we summarize the advanced characterization methods of electron spin.Then,we review the latest research advancements on the spin effect in the oxygen reduction reaction,oxygen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction.The catalytic mechanisms of spin manipulation in these four reactions are thoroughly discussed.Finally,we propose key directions for the future development of spin effects in the field of electrocatalysis.This review contributes to a deeper understanding of the micromechanisms in electrocatalytic reactions.
文摘The authors regret an inadvertent error in Fig.3a where a methyl group was drawn as an ethyl group in the trimethyl phosphate(TMP)structure,resulting in ethyl dimethylphosphate.This unintentional oversight occurred during graphic preparation.A revised structure is provided here.
基金supported by the Natural Science Foundation of Fujian Province,China(2021J06001)National Natural Science Foundation of China(22372072)National Key Research and Development Program of China(2020YFB1505800).
文摘With issues of energy security and environmental crisis intensifying,we urgently need to develop energy storage systems with high energy density and high safety.Zinc–air batteries have attracted extensive attention for their energy density,safety,and low cost,but problems with the zinc anode—such as hydrogen evolution,corrosion,passivation,dendrite proliferation,and deformation—have led to zinc–air batteries with low Coulombic efficiency and short cycle life;these remain the key obstacles hindering the batteries’further development.In this review paper,we briefly describe the reaction mechanism of zinc–air batteries,then summarize the strategies for solving the key issues in zinc anodes.These approaches are divided into three aspects:structural designs for the zinc anode;interface engineering;and electrolyte selection and optimization.We finish by offering some suggestions for future research directions to improve the zinc anode in zinc–air batteries.
基金supported by the National Natural Science Foundation of China(Youth Program,No.22309209)the Key Research and Development Program of Hunan Province(Grant No.2023GK2015)+3 种基金the Leading Telant in Science and Technological Innovation Program of Hunan Province,China(No.2022RC3049)the Tianshan Innovation Team Program of Xinjiang,China(No.2024D14001)the Natural Science Foundation of Hunan Province China(Grant No.2023JJ40709)This project was also supported by the State Key Laboratory of Powder Metallurgy,Central South University.
文摘Integrating single atoms and clusters into a unified catalytic system represents a novel strategy for enhancing catalytic performance.Compared to single-atom catalysts,those incorporating both single atoms and clusters exhibit superior catalytic activity.However,the co-construction of these systems and the mechanisms of their catalytic efficacy remain challenging and poorly understood.In this study,we synthesized a Mn–N–C catalyst featuring MnY clusters and Mn single atoms via a straightforward two-step sintering method.Y doping facilitated the formation of Mn clusters and optimized the d-band center of Mn through a unique synergy effect,thereby reducing energy barriers and enhancing the reaction kinetics.Additionally,the electron-donating ability of Y single atoms promoted the formation of unsaturated Mn–N_(₃)coordination structures,resulting in excellent oxygen reduction reaction(ORR)performance.Consequently,the MnY/NC catalyst demonstrated a half-wave potential(E_(₁/₂))of 0.90 V and maintained stability in 0.1 M KOH,outperforming both Mn/NC and Pt/C.This work underscores the potential of rare earth metal doping in transition metals to create stable single-atom and cluster systems,effectively leveraging their synergy effect for superior catalytic performance and validating the concept of the“remote synergy effect”in heterogeneous catalysis.
基金supported by the National Natural Science Foundation of China(Grant No.T2293692,21925404,22361132532,22021001)the Natural Science Foundation of Fujian Province(Grant No.2021J05193).
文摘The integration of surface plasmons with catalysis has opened a new frontier in the field of chemical energy conversion,offering unprecedented opportunities for enhancing reaction activity and selectivity.This review delves into the optical properties of plasmonic materials,the intricate mechanisms of plasmon-assisted chemical reactions(PACRs),and the fabrication of plasmonic catalysts,highlighting the significance of the structure–performance relationship.The mechanisms of PACRs are summarized to understand their synergistic contributions to reactions.The review further examines modern experimental strategies for characterizing surface plasmon resonance properties,including scanning probe microscope,in situ spectroscopy,and ultrafast laser pump-probe techniques,which provide real-time,dynamic insights into molecular interactions and structural changes with high spatial and temporal resolution.We conclude by outlining the challenges and future prospects for PACRs,emphasizing the need for innovative strategies to fully exploit the potential of PACRs for sustainable energy conversion and environmental remediation.
基金supported by the National Natural Science Foundation of China(52373087,51973235,52173091,22208331 and 62274050)Program for Leading Talents of National Ethnic Affairs Commission of China(MZR21001)+2 种基金Hubei Provincial Natural Science Foundation of China(2021CFA022)Wuhan Science and Technology Bureau(2020010601012198)Zhejiang Provincial Natural Science Foundation of China under Grant No.LZ21E020002.
文摘Bismuth vanadate(BiVO_(4))is a promising photoanode material for photoelectrochemical(PEC)water oxidation.However,its performance is greatly hindered by poor bulk and interfacial charge transfer.Herein,to address this issue,iron doped vanadyl phosphate(Fe:VOPO_(4))was grafted on molybdenum doped BiVO_(4)(Mo:BiVO_(4))for significantly enhancing charge transfer and oxygen evolution kinetics simultaneously.Consequently,the resultant Fe:VOPO_(4)/Mo:BVO_(4) photoanode exhibits a remarkable photocurrent density of 6.59 mA cm^(-2) at 1.23 V versus the reversible hydrogen electrode(VRHE)under AM 1.5G illumination,over approximately 5.5 times as high as that of pristine BiVO_(4).Systematic studies have demonstrated that the hopping activation energy of small polarons is significantly reduced due to the Mo doping,resulting in accelerated bulk charge transfer.More importantly,the deposition of Fe:VOPO_(4) promotes the interfacial charge transfer between Mo:BiVO_(4) and Fe:VOPO_(4) via the construction of V-O-V and P-O bonds,in addition to facilitating water splitting kinetics.This work provides a general strategy for optimizing charge transfer process,especially at the interface between photoanodes and cocatalysts.
基金supported by the Ministry of Science and Technology of the People's Republic of China(2022YFB2402200 and 2019YFA0705600)the National Natural Science Foundation of China(22121005,22005155,52072186,52203066,51673148 and 51678411)+5 种基金the Fundamental Research Funds for the Central Universities of China(63233017,63231002 and 63231198)the Science and Technology Plans of Tianjin,China(19PTSYJC00010)the China Postdoctoral Science Foundation Grant(2023M742135)the National Innovation and Entrepreneurship Training Program for College Students,China(202110058017)Tianjin Natural Science Foundation(23JCYBJC00660)Tianjin Enterprise Science and Technology Commissioner Project(23YDTPJC00490).
文摘Solid-state lithium battery(SSLB)is considered as one of the promising candidates for next-generation power batteries due to high safety,unprecedented energy density and favorable adaptability to high pression and temperature.However,the system of solid electrolyte(SE),as one of the most important components in SSLB,is usually plagued by clumsy ionic transport,leading to poor rate performance of the SSLBs.Herein,a unique perspective is proposed to re-examine the ion-transport behavior in lithium conductors by tracing Liþat multiscale,including microscopic,mesoscopic and macroscopic scales.The multi-scale ion-transport mechanisms and corresponding characterization techniques are analyzed in depth.Furthermore,some strategies of structure design to improve ion-transport kinetics at corresponding scales are elaborated systematically,involving the modulation of microscopic homogeneous structure,mesoscopic heterogeneous structure and macroscopic structures,etc.The proposed generalized rules for SEs are expected to construct a close link from mechanism-structure-characterization to high performances for SSLBs.
基金supported by the National Key Research and Development Program of China(2023YFB2503600)Yunnan Major Scientific and Technological Projects(grant NO.202402AF080004)+1 种基金the National Natural Science Foundation of China(22279089)the Municipal Key R&D Program of Ningbo(2023Z109).
文摘Black phosphorus(BP)anode with high capacity(2596 mAh g^(-1))and suitable lithiation potential(0.7 V vs.Li^(+)/Li)is an ideal candidate for high-energy-density and high-safety lithium-ion batteries,however,the practical implementation is greatly limited by its slow reaction kinetics and huge volume expansion.Here,inspired by nature,liquid metal(LM)is explored as a self-heal agent,which can well stabilize the BP anode through buffering the volumetric expansion and re-activating“dead P and Li x P”.Moreover,LM also acts as a good catalyst,which can adjust Li ion concentration and reduce the activation energy of delithiation reaction,thus prolonging the cycling life.Therefore,the LM modified BP/graphite(G)composite delivers an excellent high-rate performance of 1123 mAh g^(-1)at 4 C with 80.0%capacity retention after 200 cycles,a superior wide-temperature performance of 1547.5 mAh g^(-1)and 569.0 mAh g^(-1)at 50℃and-20℃,respectively.
基金supported by the National Natural Science Foundation of China(Grant No.62105238)。
文摘Full-body avatar reconstruction offers users immersive and interactive experiences in virtual space,which are crucial for the advancement of metaverse applications.However,traditional hardware solutions,reliant on optical cameras or inertial sensors,are hampered by privacy concerns,spatial limitations,high costs,and calibration challenges.Here,we propose AI-enabled smart clothing that seamlessly integrates triboelectric strain-sensing fibers(TSSFs)and AI algorithms with commercial fitness suits to achieve precise dynamic 3D reconstruction of body movement.TSSFs enable the dynamic capture of body postures and excel in sensitivity,linearity,and strain range,while maintaining mechanical stability,temperature resilience,and washability.The integrated algorithms accurately decouple posture signals—distinguishing between similar postures with the 1D-CNN algorithm,compensating for body-shape differences via a calibration algorithm,and determining spatial elements for avatar reconstruction using a decision-tree algorithm.Finally,leveraging Unity-3D,we achieve ultra-accurate dynamic 3D avatars with a joint angle error of<3.63°and demonstrate their effectiveness using VR fitness and enter-tainment applications,showing how they can offer users standardized yet engaging experiences.
基金supported by National Natural Science Foundation of China(Grant No.52002094,22479037)Guangdong Basic and Applied Basic Research Foundation(Grant No.2019A1515110756)+2 种基金Shenzhen Science and Technology Program(Grant No.JCYJ20210324121411031,JSGG202108021253804014,RCBS20210706092218040)the Shenzhen Steady Support Plan(GXWD20221030205923001,GXWD20201230155427003-20200824103000001)State Key Laboratory of Precision Welding&Joining of Materials and Structures(Grant Nos.24-Z-17,24-T-08).
文摘The Li-O_(2) battery(LOB)has attracted growing interest,including for its great potential in next-generation energy storage systems due to its extremely high theoretical specific capacity.However,a series of challenges have seriously hindered LOB development,such as sluggish kinetics during the oxygen reduction and oxygen evolution reactions(ORR/OER)at the cathode,the formation of lithium dendrites,and undesirable corrosion at the lithium metal anode.Herein,we propose a strategy based on the ultra-low loading of atomic Ni catalysts to simultaneously boost the ORR/OER at the cathode while stabilizing the Li metal anode.The resultant LOB delivers a superior discharge capacity(>16,000 mAh g^(-1)),excellent long-term cycling stability(>200 cycles),and enhanced high rate capability(>300 cycles@500 mA g^(-1)).The working mechanisms of these atomic Ni catalysts are revealed through carefully designed in situ experiments and theoretical calculations.This work provides a novel research paradigm for designing high-performance LOBs that are useable in practical applications.
基金supported by the Key Research and Development Program of Hunan Province(2023GK2015)the Science and Technology Innovation Leader Program of Hunan Province(2022RC3049).
文摘Aqueous zinc-ion batteries(ZIBs)represent a promising solution for“beyond-lithium-ion”chemistries,but certain problems hinder their further development,especially when conventional aqueous electrolytes are involved.Hydrogel polymer electrolytes(HPEs)offer opportunities to circumvent these issues.This review aims to provide a fundamental understanding of how to design better HPEs for high-performing ZIBs,through critically analyzing the recent literature.Concerns regarding HPEs’mechanical,interfacial,and electrochemical characteristics are addressed,followed by in-depth insights into their underlying mechanisms.Possibilities for practical applications of HPEs are also discussed.
基金supported by the National Natural Science Foundation of China(22278091)the Guangxi Natural Science Foundation of China(2023GXNSFFA026009).
文摘Wearable tactile sensing systems with bionic designs holds significant promise for environmental interactions and human–machine communication.Triboelectric sensing technology plays a vital role in acquiring and quantifying tactile signals.Conventional elastic sensing materials,however,lack damping performance and are easily damaged by vibrations,leading to sensor failure.To address this challenge,our study proposes a highly damping triboelectric gel based on a hydrogen bonding assisted microphase separation strategy.In microphase separation,the soft phase provides the viscoelasticity needed for the gel,while the hard phase dissipates shock energy.This energy dissipation mechanism enables the gel to achieve excellent damping performance(tanδ=0.68 at 1Hz),skin-like softness(Young’s modulus of 130 kPa),and stretchability(>900%).The resulting self-damping tactile patch effectively absorbs and dissipates external vibrations,ensuring a stable and reliable wearable tactile sensing device.This work provides new insights into the application of triboelectric gels in wearable electronics.
基金supported by the National Key R&D Program of China(2021YFB2402002)Beijing Natural Science Foundation(Grant No.L223013)the National Natural Science Foundation of China(Grant No.52272359 and 52376167).
文摘Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era.Different from traditional methods,this work proposes a hybrid framework for rapid and accurate degradation diagnosis at the electrode level combining both deep learning,which is used to rapidly and robustly predict polarization-free incremental capacity analysis(ICA)curves in minutes,and physical modeling,which is used to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves.Only measured charging current and voltage signals are used.Results demonstrates that 11 points collected at any starting state-of-charge(SOC)in a minimum of 2.5 minutes are sufficient to obtain reliable ICA curves with a mean root mean square error(RMSE)of 0.2774 Ah/V.Accordingly,battery status can be accurately elevated based on their degradation at both macro and electrode levels.Through transfer learning,such a method can also be adapted to different battery chemistries,indicating the enticing potential for wide applications.
基金the National Key R&D Program of China(No.2021YFB4000200)the National Natural Science Foundation of China(No.22232004)+1 种基金the Instrument Developing Project of the Chinese Academy of Sciences,the Jilin Province Development and Reform Commission Program(2023C032-6)the Jilin Province Science and Technology Development Program(No.20210301008GX,YDZJ202202CXJD011,20210502002ZP)for financial support.
文摘The development of low-cost and efficient electrocatalysts for oxygen evolution reaction(OER)in acid electro-lytes is critical to the widespread implementation of proton electrolyte membrane water electrolyzers(PEMWE)towards carbon neutralization.Noble metal Ir-and Ru-based materials are state-of-the-art catalysts but still suffer from prohibitive price and scarcity.In this context,a variety of noble metal-free catalysts have been developed to decrease the cost of PEMWE.In this review,we first summarize the activity expression mechanism and stability issues for non-precious metal catalysts,highlighting the origins of performance degradation and the possible mitigation strategies.Then,we systematically review several recently developed noble metal-free catalysts,focusing on the design rationale and the structure-performance relation.Finally,the development prospects of non-noble metal catalysts are prospected,with the potential challenges for practical applications presented.
基金supported by the National Natural Science Foundation of China(grant numbers 52374410,22209006)the Natural Science Foundation of Shandong Province(grant numbers ZR2022QE009)+3 种基金Beijing Natural Science Foundation(grant numbers Z220021)the National Key R&D Program of China(grant numbers 2022YFB3305400)the Joint Funds of the National Natural Science Foundation of China(grant numbers U2130204)Beijing Outstanding Young Scientists Program(grant numbers BJJWZYJH01201910007023).
文摘In the development of sustainable lithium-ion batteries,achieving the efficient and cost-effective recycling of all components,particularly spent graphite(SG)anodes,has become a critical requirement.While considerable ef-forts have been devoted to recovering and reusing SG materials under conventional conditions,limited attention has been given to recycling under extreme conditions.This review systematically elucidates the main failure mechanisms of graphite anodes,including lithium plating and dendrite formation,solid electrolyte interface film failure,structural degradation,and current collector corrosion,with a particular focus on low-temperature and fast-charging conditions.As a contribution toward optimizing resource utilization,this review comprehensively summarizes the industrial perspective on strategies for recycling SG anodes,which aim to produce high-purity regenerated graphite(RG)powders.We also analyze current methods for modifying RG,such as structural reconstruction and surface reconditioning,to bring added value to modified RG materials.A detailed examination of the technical challenges in SG recycling and RG upgrading is presented,offering guidance for the future development of graphite upcycling technologies.This review also provides valuable insights into achieving high efficiency,intelligence,and sustainability in graphite utilization.
基金supported by the National Natural Science Foundation of China(22209006,21935001,22205068)the Natural Science Foundation of Shandong Province(ZR2022QE009)+2 种基金Fundamental Research Funds for the Central Universities(buctrc202307)the National Key Beijing Natural Science Foundation(Z210016)the Fundamental Research Funds for the Central Universities,and the long-term subsidy mechanism from the Ministry of Finance and the Ministry of Education of China,and the“CUG Scholar”Scientific Research Funds at China University of Geosciences(Wuhan)(Project No.2022118).
文摘The invention of aqueous Zn batteries(AZBs)traces back to the eighteenth century.Recently,however,AZBs have been undergoing a renaissance due to the urgent need for renewable energy storage devices that are intrinsically safe,inexpensive,and environmentally benign.The escalating demand for high-energy,fast-charging AZBs,particularly in grid-scale energy storage systems,necessitates a profound exploration of the fundamental aspects of electrode chemistries.In particular,a comprehensive understanding from the viewpoints of thermodynamics and kinetics is crucial,with the aim of advancing the development of next-generation AZBs that have high power and energy densities.However,clarification about the fundamental issues in AZB chemistry has yet to be ach-ieved.This review offers a thorough exploration of the thermodynamics and dynamic mechanisms at the anode and cathode,with the aim of helping researchers achieve high-performance AZBs.The inherent challenges and corresponding strategies related to electrode thermodynamic and dynamic optimization are summarized,fol-lowed by insights into future directions for developing high-energy,fast-charging AZBs.We conclude by considering the future prospects for AZBs and offering recommendations for making further advancements in discovering new redox chemistries,optimizing electrode architectures,and achieving integrated battery designs,all of which are considered essential and time-sensitive for making high-energy,fast-charging,and durable AZBs a reality.
基金supported by the National Natural Science Foundation of China(52402302,52250710680)High-end Foreign Experts Recruitment Plan of China(G2023016009L)+3 种基金Zhejiang Provincial Natural Science Foundation of China(LQ24E020001)Key Research and Development Program of Zhejiang Province(2024C01057,2023C01232)Science and Technology Plan Project of Wenzhou Municipality(ZG2022032)The Natural Science Foundation of Changsha(kq2402017).
文摘Hard carbon(HC)anodes in sodium-ion batteries(SIBs)are prized for their high capacity,durability,costefficiency,environmental sustainability,and safety.The metallic ash elements in HCs inevitably affect the overall performance of SIBs,however,the unclear role of metallic ash elements during carbonization and the electrochemical sodium storage process presents challenges for advancing HC design concepts.In this review,the traditional role of metallic ash element realized in the past and the deep understanding by a new sight from the view of intrinsic types in precursor matrix are initially introduced.Subsequently,the effect of catalyzing graphitization degree,constructing pore structure,tuning SEI formation and tailoring defects of the HCs regulated by extrinsic factors introduced through experimental conditions in recent years are comprehensively summarized.Additionally,future development prospects and perspectives on the research about metallic ash element in HC are also briefly outlined.It is believed that this review can deliver noteworthy viewpoints by introducing metallic ash elements,for the continued development of adjusting the microstructure of HCs at the nanoscale to actualize highperformance SIBs.
基金supported by the National Natural Science Foundation of China(52203215)the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(Grant No.NY225035).
文摘Affordable,easily recycled organics with electroactive centers have drawn attention in the pursuit of high-performance aqueous zinc organic batteries(AZOBs).However,intrinsic barriers such as high solubility,unde-sirable potential,and inferior conductivity hinder their further development.To this end,we have designed an advanced cathode material for AZOBs,comprising an n-type polymer with a three-dimensional(3D)building block(HAT-TP)formed by polymerizing 2,3,6,7,10,11-hexacyano-1,4,5,8,9,12-hexazepenanthrene(HAT-CN)and 3D 2,3,6,7,14,15-hexaaminotriptycene(THA-NH 2).The introduction of a 3D architecture not only bolsters the insolubility but also exposes redox-active sites for cation coordination,while the material's extended conjugated system promotes electronic delocalization to increase the redox potential and conductivity.As a result,a HAT-TP battery exhibits a notable initial discharge voltage of 1.32 V at 0.1 A g^(-1),followed by a midpoint voltage of 1.17 V.Remarkably,an ultrastable capacity retention ratio of up to 93.4%is achieved,even after 40,000 cycles at 5 A g^(-1).Theoretical simulations reveal that the elevated discharge potential results from the strong electronic delocalization of HAT-TP,which improves the affinity with cations.Ex situ characterizations and theoretical calculations verify that the reversible Zn^(2+)/H^(+)co-storage mechanism involves only electroactive C=N sites and the best possible coordination paths between them.
